期刊
ACS ENERGY LETTERS
卷 5, 期 7, 页码 2444-2451出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsenergylett.0c00959
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资金
- National Natural Science Foundation of China [51801235, 11875258, 11505187, 51374255, 51802356, 51572299]
- InnovationDriven Project of Central South University [2018CX004]
- Central South University [502045005]
- Fundamental Research Funds for the Central Universities [WK2310000066, WK2060190081, WK3430000005]
- Natural Science Foundation of Hunan Province [2020JJ5690]
- Postdoctoral Science Foundation of China [2019M652797]
- Opening Sharing Fund for the Large-scale Instruments and Equipment of Central South University [CSUZC202001]
Developing low-cost Cu-based photocatalysts is a promising strategy to boost catalytic activity for nitrogen (N-2) photofixation, but it remains a challenge. Herein, we successfully applied porous CuFe to construct plasmon-assisted Cu-based photocatalysts in N-2 photofixation via plasmonic catalysis. Surface Fe atoms were regarded as the active sites to efficiently adsorb and activate N-2, while Cu frameworks generated hot electrons by surface plasmon resonance (SPR). Impressively, porous Cu96Fe4 attained an NH3 production rate of 342 mu mol.g(cat.)(-1).h(-1) in N-2 photofixation without any sacrificial agents. More importantly, porous Cu96Fe4 also displayed excellent stability by maintaining similar to 100% initial activity after 10 cycles. Further mechanistic studies revealed that the valence state and coordination numbers of Fe atoms in porous Cu96Fe4 increased during catalytic process, indicating the formation of a surface nitrogen-containing complex. In addition, the reaction barrier significantly decreased because of the efficient polarization of N-2 over Fe atoms.
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